Transformation kinetics of biochemically active compounds in low-pressure UV Photolysis and UV/H2O2 advanced oxidation processes

被引:172
作者
Baeza, Carolina [2 ]
Knappe, Detlef R. U. [1 ]
机构
[1] N Carolina State Univ, Dept Civil Construct & Environm Engn, Raleigh, NC 27695 USA
[2] Univ Concepcion, Environm Sci Ctr EULA Chile, Concepcion, Chile
基金
美国国家科学基金会;
关键词
Antibiotics; Endocrine disrupting chemicals; Pharmaceuticals; Photooxidation; Quantum yield; WATER-TREATMENT PROCESSES; SIMULATED DRINKING-WATER; RATE CONSTANTS; HETEROCYCLIC GROUPS; PHOTOCHEMICAL FATE; MIGRATION BEHAVIOR; HYDROXYL RADICALS; NATURAL-WATERS; SULFA DRUGS; WASTE-WATER;
D O I
10.1016/j.watres.2011.05.039
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Factors controlling photolysis and UV/H2O2 photooxidation rates of the biochemically active compounds (BACs) sulfamethoxazole, sulfamethazine, sulfadiazine, trimethoprim, bisphenol A, and diclofenac were determined. Experiments were conducted with a quasi-collimated beam apparatus equipped with low-pressure UV lamps. The effects of pH, H2O2 concentration, and background water matrix (ultrapure water, lake water, wastewater treatment plant effluent) on BAC transformation rates were evaluated. For the sulfa drugs, solution pH affected direct photolysis rates but had little effect on the hydroxyl radical oxidation rate. For sulfamethoxazole, the neutral form photolyzed more easily than the anionic form while the reverse was the case for sulfamethazine and sulfadiazine. For trimethoprim, the hydroxyl radical oxidation rate was higher for the cationic form (pH 3.6) than for the neutral form (pH 7.85). Quantum yields and second order rate constants describing the reaction between the hydroxyl radical and BACs were determined and used together with background water quality data to predict fluence-based BAC transformation rate constants (k'). For both the lake water and wastewater treatment plant effluent matrices, predicted k' values were generally in good agreement with experimentally determined k' values. At typical UV/H2O2 treatment conditions (fluence = 540 mJ cm(-2), H2O2 dose = 6 mg L-1), BAC transformation percentages in North Carolina lake water ranged from 43% for trimethoprim to 98% for diclofenac. In wastewater treatment plant effluent, BAC transformation percentages were lower (31-97%) at the same treatment conditions because the hydroxyl radical scavenging rate was higher. (C) 2011 Elsevier Ltd. All rights reserved.
引用
收藏
页码:4531 / 4543
页数:13
相关论文
共 33 条
[1]   Removal of antibiotics from surface and distilled water in conventional water treatment processes [J].
Adams, C ;
Wang, Y ;
Loftin, K ;
Meyer, M .
JOURNAL OF ENVIRONMENTAL ENGINEERING-ASCE, 2002, 128 (03) :253-260
[2]  
Alexy R., 2006, Organic pollutants in the water cycle, P65
[3]   Modeling of photooxidation of acetamide herbicides in natural waters by UV radiation and the combinations UV/H2O2 and UV/O3 [J].
Benitez, FJ ;
Acero, JL ;
Real, FJ ;
Maya, C .
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY, 2004, 79 (09) :987-997
[4]  
Bolton J.R., 2001, ULTRAVIOLET APPL HDB, VSecond
[5]   Fundamental photochemical approach to the concepts of fluence (UV dose) and electrical energy efficiency in photochemical degradation reactions [J].
Bolton, JR ;
Stefan, MI .
RESEARCH ON CHEMICAL INTERMEDIATES, 2002, 28 (7-9) :857-870
[6]   Standardization of methods for fluence (UV dose) determination in bench-scale UV experiments [J].
Bolton, JR ;
Linden, KG .
JOURNAL OF ENVIRONMENTAL ENGINEERING-ASCE, 2003, 129 (03) :209-215
[7]   Triplet-sensitized photodegradation of sulfa drugs containing six-membered heterocyclic groups:: Identification of an SO2 extrusion photoproduct [J].
Boreen, AL ;
Arnold, WA ;
McNeill, K .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (10) :3630-3638
[8]   Photochemical fate of sulfa drugs in the aquatic environment: Sulfa drugs containing five-membered heterocyclic groups [J].
Boreen, AL ;
Arnold, WA ;
McNeill, K .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2004, 38 (14) :3933-3940
[9]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[10]   Phototransformation of selected pharmaceuticals during UV treatment of drinking water [J].
Canonica, Silvio ;
Meunier, Laurence ;
Von Gunten, Urs .
WATER RESEARCH, 2008, 42 (1-2) :121-128